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With one foot planted in Harvard Yard, the other among scientists in the Soviet Union, Paul Doty became a leading adviser to successive presidential administrations on nuclear arms control as he bridged the intellectual divide during the Cold War.

As founder of what is now the Belfer Center for Science and International Affairs at Harvard, he also nurtured a generation of policy makers who have helped shape nonproliferation accords. Its graduates have continued, into the Obama administration, to advise world leaders on the most complex, delicate, and dangerous aspects of science and technology.

“Paul had a vision of the role of science in the service of international security, and today so many of his apprentices are working to realize that vision,’’ Ashton B. Carter, deputy secretary of defense, wrote in an e-mail. “However, we could work a lifetime and still not repay all that Paul gave to us with his leadership and, most importantly, his friendship. He will be beyond missed.’’

Dr. Doty, director emeritus of the Belfer Center and the Mallinckrodt Professor Emeritus of Biochemistry at Harvard, died of congestive heart failure in his Cambridge home yesterday. He was 91.

While offering nuclear arms advice to secretaries of state and defense, members of Congress, and presidential administrations from Dwight D. Eisenhower to Jimmy Carter, Dr. Doty kept his day job as a scientist and professor who sensed the need to break new ground at Harvard.

In the late 1960s, he launched the department of biochemistry and molecular biology, which was remarkable for the array of talent he brought into his fold. Among his initial faculty appointments, three were awarded Nobel Prizes and 14 of his research students went on to be elected to the National Academy of Sciences. Dr. Doty was elected to the academy in the late 1950s.

“Paul was a great picker of people with talent and promise, but he was also a great mentor in encouraging their development,’’ said Graham Allison, current director of the Belfer Center.

Through his work in academia and arms control, Dr. Doty “led parallel lives,’’ said Dr. Dorothy Zinberg, a lecturer in science, technology, and public policy at the Belfer Center who has known Dr. Doty since the 1960s. “The people in his laboratory wondered where he was when he was off doing arms control, and the people in arms control wondered where he was when he was doing biochemistry.’’

Those lives, however, “were closely linked,’’ said Albert Carnesale, chancellor emeritus and professor of public policy and engineering at the University of California at Los Angeles and a former provost at Harvard.

“Paul led a distinguished life as a chemist; there’s no question,’’ Carnesale said. “And he also led a distinguished life in public policy. And he trained a generation of people who are like that.’’

The linkage could be seen in the name of the center Dr. Doty created. To him, science and international affairs were easily intertwined.

In 1957, when Dr. Doty was leader of the Federation of American Scientists, he was invited to Pugwash, Nova Scotia, for what became known as the Pugwash Conferences, where scientists met to address concerns about controlling nuclear arms and preventing a world war.

Dr. Doty visited the Soviet Union a few dozen times, meeting with scientists there who included Andrei Sakharov.

Sakharov would later be awarded the Nobel Peace Prize, and the Pugwash Conferences shared the Peace Prize in 1995.

The Belfer Center, however, had its own widening ripple effect. In the early 1970s, Dr. Doty persuaded McGeorge Bundy, a former national security adviser who was then president of the Ford Foundation, to use the foundation’s funding to help create a center for science and international affairs at Harvard.

The center is now part of the John F. Kennedy School of Government. Among those who studied or worked at the center are two members of the Obama administration, Ashton Carter and John P. Holdren, assistant to President Obama for science and technology.

“Paul Doty was a giant in science and a pioneer in building institutions for communicating relevant insights from science to policy makers,’’ Holdren said in a statement released by Harvard. “He was a mentor and an inspiration to me and many others, one of the wisest and warmest people I’ve had the privilege to know.’’

At Dr. Doty’s 90th birthday celebration last year, Carter said that “Paul taught us how to combine the spirit of science and the life of the mind with practical affairs.’’

Addressing Dr. Doty, he said there “are generations of young people who are now doing what you wanted them to do, who would not be where they are were it not for the Center for Science and International Affairs at the Kennedy School, at Harvard.’’

Also at last year’s celebration was James D. Watson, who shared a Nobel Prize in 1962 for codiscovering the structure of DNA. Watson was among the scientists Dr. Doty recruited to Harvard’s biochemistry department.

Looking around the scientists gathered at the celebration, Watson said, “I think we all owe Paul our jobs,’’ and added: “[Dr. Doty] was my mentor. There was never a finer person on the Harvard faculty.’’

An only child, Paul Mead Doty was born in Charleston, W.Va., and grew up in Chicora, Pa.

He later would tell the story of how he was so much more advanced in chemistry than anyone else at his high school that the teacher ultimately asked him to teach the class.

Dr. Doty graduated from Pennsylvania State University in 1941 with a bachelor’s in chemistry and received a doctorate in chemistry from Columbia University in 1944.

During his graduate studies, he also worked on the Manhattan Project, developing the first atomic bomb, and credited the experience with laying the groundwork for his future work on arms control.

Dr. Doty’s first marriage, to Margaretta Gravatt, ended in divorce. She died in 2005.

He married Helga Boedtker, and the two worked together running a laboratory at Harvard. She died in 2001.

A service will be announced for Dr. Doty, who leaves a son, Gordon of Cambridge; three daughters, Marcia and Rebecca, both of Franklin, N.C., and Katherine of San Francisco; and three grandchildren.

“He was obviously quite proud of the Belfer Center and was thrilled that so many of its alumni now have the opportunity to make a difference,’’ Allison said. “He remained an active participant here at the center, coming to our internal board lunches until the past month.’’

Dr. Doty also “had a lovely quiet sense of humor,’’ Zinberg said. She added that her friend and colleague also approached work in a way that was unusual in fields populated by scientists with blazing talent and soaring egos. “Jim Watson once said to him, ‘Your strength was in never wanting power.’ ’’